Date of Degree

9-2016

Document Type

Dissertation

Degree Name

Ph.D.

Program

Chemistry

Advisor

George John

Committee Members

Akira Kawamura

Raymond Tu

Charles Maldarelli

Subject Categories

Materials Chemistry

Keywords

gelators, gels, sustainability, green chemistry, smart materials, mechanochemistry

Abstract

Though molecular gelators may by synthesized and formulated into gels following a variety of methods, it should serve that the most valued methods may utilize renewable and waste resources and follow sustainable procedures. Molecular gelators are systems capable of structuring liquids into solid-like materials and they represent a class of surfactant and amphiphilic materials which posses the capability to be not only useful in their ability to form gels, but multifunctional in the ability to respond smartly to a variety of stimuli. Thus there is an interest in the development of sustainable molecular gelators capable of being applied to applications, which may have been previously linked to gels, or more interestingly those with which gels have not yet been applied.

The use of naturally occurring starting materials in the form of renewable resources serves to inspire biomimetic species which allow for the simultaneous development of materials for applied research, while affording researchers the opportunity to study the importance of non-covalent intermolecular interaction and their roles in natural molecules. Deriving these gelators from the basic primary metabolites may help unveil the nature of these forces in their assembly, and most excitingly their function.

In an effort to explore the functionality and utility of biobased gelled supramolecular systems, two gelators, one primarily structuring organic solvents, and the other a hydrogelator are discussed from a synthetic point of view and characterized for their non-covalent interactions. Enzymatic catalysis is performed to afford these species in high yields, allowing for the eventual potential commercialization of these gelators through benign means. In addition to the gelator characterization, the resultant composite gels are studied for their mechanical properties, but of most interest their ability to be defined as smart materials in their response to shear, heat and light. Lastly these materials are examined for their application to three different areas of current interest: healthful edible oil structuring, next-generation gelled fuels, and radiation sensing gels. This study should serve as a rigorous investigation not only in the sustainable development of functional value-added chemicals, but their formulation and processing into value-added materials.

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